RESUMEN
The radionuclides 43Sc, 44g/mSc, and 47Sc can be produced cost-effectively in sufficient yield for medical research and applications by irradiating natTi and natV target materials with protons. Maximizing the production yield of the therapeutic 47Sc in the highest cross section energy range of 24-70 MeV results in the co-production of long-lived, high-γ-ray-energy 46Sc and 48Sc contaminants if one does not use enriched target materials. Mass separation can be used to obtain high molar activity and isotopically pure Sc radionuclides from natural target materials; however, suitable operational conditions to obtain relevant activity released from irradiated natTi and natV have not yet been established at CERN-MEDICIS and ISOLDE. The objective of this work was to develop target units for the production, release, and purification of Sc radionuclides by mass separation as well as to investigate target materials for the mass separation that are compatible with high-yield Sc radionuclide production in the 9-70 MeV proton energy range. In this study, the in-target production yield obtained at MEDICIS with 1.4 GeV protons is compared with the production yield that can be reached with commercially available cyclotrons. The thick-target materials were irradiated at MEDICIS and comprised of metallic natTi, natV metallic foils, and natTiC pellets. The produced radionuclides were subsequently released, ionized, and extracted from various target and ion source units and mass separated. Mono-atomic Sc laser and molecule ionization with forced-electron-beam-induced arc-discharge ion sources were investigated. Sc radionuclide production in thick natTi and natV targets at MEDICIS is equivalent to low- to medium-energy cyclotron-irradiated targets at medically relevant yields, furthermore benefiting from the mass separation possibility. A two-step laser resonance ionization scheme was used to obtain mono-atomic Sc ion beams. Sc radionuclide release from irradiated target units most effectively could be promoted by volatile scandium fluoride formation. Thus, isotopically pure 44g/mSc, 46Sc, and 47Sc were obtained as mono-atomic and molecular ScF 2+ ion beams and collected for the first time at CERN-MEDICIS. Among all the investigated target materials, natTiC is the most suitable target material for Sc mass separation as molecular halide beams, due to high possible operating temperatures and sustained release.
RESUMEN
Sulfonated poly(ether ether ketone) (SPEEK) materials are promising candidates for replacing Nafion™ in applications such as proton exchange membrane (PEM) and direct methanol fuel cells. SPEEK membranes have several advantages such as low cost, thermal and radiation stability and controllable physicochemical and mechanical properties, which depend on the degree of sulfonation (DS). Commercial PEEK was homogenously sulfonated up to a DS of 60-90% and the membranes were prepared using a solvent casting method. Part of the samples were irradiated with a 10 MeV electron beam up to a 500 kGy dose to assess the ionizing radiation-induced effects. Both non-irradiated and irradiated membranes were characterized by Fourier Transformation infrared (FT-IR) spectroscopy, thermogravimetric analysis (TGA), proton nuclear magnetic resonance (1H-NMR) spectroscopy, electrochemical impedance analysis and, for the first time for non-irradiated membranes, by spectrophotometric analysis with Cr(III). The above-mentioned methods for application for DS assessment were compared. The aim of this study is to compare different methods used for the determination of the DS of SPEEK membranes before and after high-dose irradiation. It was observed that irradiated membranes presented a higher value of DS. The appearance of different new signals in 1H-NMR and FT-IR spectra of irradiated membranes indicated that the effects of radiation induced changes in the structure of SPEEK materials. The good correlation of Cr(III) absorption and SPEEK DS up to 80% indicates that the spectrophotometric method is a comparable tool for the characterization of SPEEK membranes.
